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US4195123A - Non-aqueous electrolyte lithium battery with improved storage life - Google Patents

Non-aqueous electrolyte lithium battery with improved storage life Download PDF

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Publication number
US4195123A
US4195123A US06/002,090 US209079A US4195123A US 4195123 A US4195123 A US 4195123A US 209079 A US209079 A US 209079A US 4195123 A US4195123 A US 4195123A
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United States
Prior art keywords
solvent
active material
negative electrode
lead
lithium
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Expired - Lifetime
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US06/002,090
Inventor
Yves Jumel
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SAFT Societe des Accumulateurs Fixes et de Traction SA
Honeywell International Inc
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SAFT Societe des Accumulateurs Fixes et de Traction SA
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Assigned to ALLIED CORPORATION reassignment ALLIED CORPORATION CHANGE OF NAME (SEE DOCUMENT FOR DETAILS). Assignors: ALLIED CHEMICAL CORPORATION
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
    • H01M4/40—Alloys based on alkali metals
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M6/00—Primary cells; Manufacture thereof
    • H01M6/14—Cells with non-aqueous electrolyte
    • H01M6/16—Cells with non-aqueous electrolyte with organic electrolyte

Definitions

  • the present invention relates to an electrochemical cell having a non-aqueous electrolyte, and more particularly to a primary cell whose positive active material is very slightly soluble in the solvent of the electrolyte. This is the case, for example, with lithium lead oxide cells using dioxolane as their electrolyte solvent.
  • the dissolved lead oxide moves towards the negative electrode where it is reduced to lead which is deposited on the lithium.
  • the quantity of lead thus lost is small, so this would not be a great disadvantage if it were not for the occurrence of the following phenomenon: instead of spreading out regularly over the surface of the lithium electrode, the lead is deposited only at certain privileged points. This selective deposition causes dendrites to develop perpendicularly to the surface of the electrode at these points. Eventually these dendrites may perforate the separator and come into contact with the positive electrode, thus short-circuiting the cell.
  • the invention mitigates this disadvantage.
  • an electrochemical cell including a non-aqueous electrolyte which comprises a solute and at least one solvent; a lithium negative electrode; and a positive active material which is slightly soluble in said solvent; wherein the surface of the negative electrode is alloyed with at least one of the following metals: lead, tin, antimony and silver.
  • lead is used when the positive active material is lead oxide and in particular when said solvent is dioxolane.
  • “Surface of the negative electrode” means a very thin layer, in the order of a few hundredths of a millimeter when the thickness of the negative electrode lies between 0.5 mm and 1.5 mm.
  • the invention also provides a method of manufacturing such a negative electrode, in accordance with which a sheet of the said metal is pressed against the surface of the electrode, said sheet having a thickness in the order of a few hundredths of a millimeter, e.g. lying between 0.005 mm and 0.03 mm.
  • the minimum desirable pressure for pressing the metal against the electrode is 20 kg/cm 2 .
  • the minimum desirable pressure is greater.
  • a thin layer of the said metal may also be deposited on the lithium surface either by vapor deposition or by spraying and the metal-plated lithium is then pressed (e.g., rolled) to alloy the metal to the lithium, using a pressure of the same order of magnitude as that used in the previous method, although the minimum workable pressure is lower.
  • FIGURE is a diagrammatic cross-section of the cell.
  • Such a cell includes a casing whose outside diameter is in the order of 10 mm and whose height is 5 mm and which is formed by a cap 7 and a cup 1 made of nickel-plated steel or stainless steel.
  • the cup and the cap are separated by a seal 8 made of a plastic material for sealing and for electrically insulating the cup from the cap.
  • the positive cup 1 contains a powdered active material 2, for example lead oxide, to which an electron conductor is added in a known way together with a binding agent, if needed.
  • the active mass is compressed in the cup 1, which includes a metal ring 9 made of nickel-plated steel or stainless steel, said metal ring being used to contain the active material and to reinforce the support of the seal 8 against the pressure of the cup 1 while the lip of the cup 1 is being bent back over the seal 8.
  • the negative cap 7 contains a lithium pellet 5 including a current collector 6 constituted by a nickel-plated steel or stainless steel grid welded to the cap.
  • the thickness of the lithium electrode lies between 0.5 mm and 1.5 mm.
  • the surface of the electrode situated on the positive electrode side is alloyed with lead, the thickness of the layer 10 of the alloy lying preferably between approximately 0.005 mm and 0.03 mm.
  • the positive and negative electrodes are separated by a paper barrier 3 and layers of cellulose felt 4 impregnated with electrolyte.
  • the electrolyte includes at least one non-aqueous solvent such as dioxolane.
  • the alloy layer 10 can be obtained very simply by pressing a very thin sheet of lead onto the surface of the lithium electrode preferably with a pressure of about 20 kg/cm 2 .
  • the lead then diffuses into the lithium and a genuine alloy is formed.
  • the metallic lead reduced from the lead oxide coming from the positive electrode is then deposited regularly over the whole surface of the negative electrode, without being concentrated at certain points as in the case of pure lithium electrode.
  • the surface alloy does not hinder the discharge of the cell.
  • the invention is not limited to the embodiment which has just been described.
  • the lead alloy can be replaced by an alloy of tin, antimony, and/or silver.
  • the invention applies to lithium cells which have positive active materials which are very slightly soluble in the solvent of the electrolyte, and not only to cells using lead oxide as the positive active material.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Primary Cells (AREA)
  • Battery Electrode And Active Subsutance (AREA)
  • Secondary Cells (AREA)
  • Saccharide Compounds (AREA)

Abstract

In an electrochemical cell having a non-aqueous electrolyte which comprises a solute and at least one solvent, a lithium negative electrode, and a positive active material of said cell which is slightly soluble in said solvent, the surface of the negative electrode is alloyed with at least one metal chosen from the group consisting of lead, tin, antimony and silver, to prevent selective localized deposition onto the lithium electrode of metal reduced from the positive active material during storage. The improvement is particularly applicable to cells in which the positive active material is lead oxide and said solvent is dioxolane.

Description

The present invention relates to an electrochemical cell having a non-aqueous electrolyte, and more particularly to a primary cell whose positive active material is very slightly soluble in the solvent of the electrolyte. This is the case, for example, with lithium lead oxide cells using dioxolane as their electrolyte solvent.
During storage of such a cell, the dissolved lead oxide moves towards the negative electrode where it is reduced to lead which is deposited on the lithium. The quantity of lead thus lost is small, so this would not be a great disadvantage if it were not for the occurrence of the following phenomenon: instead of spreading out regularly over the surface of the lithium electrode, the lead is deposited only at certain privileged points. This selective deposition causes dendrites to develop perpendicularly to the surface of the electrode at these points. Eventually these dendrites may perforate the separator and come into contact with the positive electrode, thus short-circuiting the cell.
The invention mitigates this disadvantage.
It provides an electrochemical cell including a non-aqueous electrolyte which comprises a solute and at least one solvent; a lithium negative electrode; and a positive active material which is slightly soluble in said solvent; wherein the surface of the negative electrode is alloyed with at least one of the following metals: lead, tin, antimony and silver.
Advantageously, lead is used when the positive active material is lead oxide and in particular when said solvent is dioxolane.
"Surface of the negative electrode" means a very thin layer, in the order of a few hundredths of a millimeter when the thickness of the negative electrode lies between 0.5 mm and 1.5 mm.
The invention also provides a method of manufacturing such a negative electrode, in accordance with which a sheet of the said metal is pressed against the surface of the electrode, said sheet having a thickness in the order of a few hundredths of a millimeter, e.g. lying between 0.005 mm and 0.03 mm. For an electrode of 1 cm2 surface area, the minimum desirable pressure for pressing the metal against the electrode is 20 kg/cm2. For electrodes of greater surface area the minimum desirable pressure is greater.
Although this method is the preferred method, a thin layer of the said metal may also be deposited on the lithium surface either by vapor deposition or by spraying and the metal-plated lithium is then pressed (e.g., rolled) to alloy the metal to the lithium, using a pressure of the same order of magnitude as that used in the previous method, although the minimum workable pressure is lower.
One example of a button-type cell in accordance with the invention will be described hereinbelow with reference to the single accompanying FIGURE, which is a diagrammatic cross-section of the cell.
Such a cell includes a casing whose outside diameter is in the order of 10 mm and whose height is 5 mm and which is formed by a cap 7 and a cup 1 made of nickel-plated steel or stainless steel. The cup and the cap are separated by a seal 8 made of a plastic material for sealing and for electrically insulating the cup from the cap. The positive cup 1 contains a powdered active material 2, for example lead oxide, to which an electron conductor is added in a known way together with a binding agent, if needed. The active mass is compressed in the cup 1, which includes a metal ring 9 made of nickel-plated steel or stainless steel, said metal ring being used to contain the active material and to reinforce the support of the seal 8 against the pressure of the cup 1 while the lip of the cup 1 is being bent back over the seal 8. The negative cap 7 contains a lithium pellet 5 including a current collector 6 constituted by a nickel-plated steel or stainless steel grid welded to the cap. The thickness of the lithium electrode lies between 0.5 mm and 1.5 mm. The surface of the electrode situated on the positive electrode side is alloyed with lead, the thickness of the layer 10 of the alloy lying preferably between approximately 0.005 mm and 0.03 mm.
The positive and negative electrodes are separated by a paper barrier 3 and layers of cellulose felt 4 impregnated with electrolyte. The electrolyte includes at least one non-aqueous solvent such as dioxolane.
In accordance with the invention the alloy layer 10 can be obtained very simply by pressing a very thin sheet of lead onto the surface of the lithium electrode preferably with a pressure of about 20 kg/cm2. The lead then diffuses into the lithium and a genuine alloy is formed. During subsequent storage of the cell, the metallic lead reduced from the lead oxide coming from the positive electrode is then deposited regularly over the whole surface of the negative electrode, without being concentrated at certain points as in the case of pure lithium electrode.
The surface alloy does not hinder the discharge of the cell.
The invention is not limited to the embodiment which has just been described. The lead alloy can be replaced by an alloy of tin, antimony, and/or silver. The invention applies to lithium cells which have positive active materials which are very slightly soluble in the solvent of the electrolyte, and not only to cells using lead oxide as the positive active material.

Claims (5)

I claim:
1. An electrochemical cell including a lithium negative electrode; a non-aqueous electrolyte which comprises a solute and at least one organic solvent; and a positive electrode spaced from the negative electrode, the positive electrode having a positive active material which is slightly soluble in said solvent; wherein the improvement comprises:
only the surface of the negative electrode being alloyed with at least one metal selected from the group formed by lead, tin, antimony and silver.
2. A cell according to claim 1, wherein the alloy layer has a thickness in the order of a few hundredths of a millimeter.
3. A cell according to claim 1 wherein the thickness of the alloy layer is between approximately 0.005 and 0.03 mm.
4. A cell according to claim 1, wherein said positive active material comprises lead oxide.
5. A cell according to claim 1, 2 or 3, wherein said solvent is dioxolane.
US06/002,090 1978-01-10 1979-01-09 Non-aqueous electrolyte lithium battery with improved storage life Expired - Lifetime US4195123A (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
FR7800507A FR2414253A1 (en) 1978-01-10 1978-01-10 NON-AQUEOUS ELECTROLYTE ELECTROCHEMICAL GENERATOR WITH IMPROVED CONSERVATION
FR7800507 1978-01-10

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US4195123A true US4195123A (en) 1980-03-25

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US (1) US4195123A (en)
AU (1) AU518526B2 (en)
BE (1) BE873068A (en)
BR (1) BR7900113A (en)
CA (1) CA1114447A (en)
CH (1) CH630494A5 (en)
DE (1) DE2900087C3 (en)
DK (1) DK9379A (en)
ES (1) ES476726A1 (en)
FR (1) FR2414253A1 (en)
GB (1) GB2013020B (en)
IT (1) IT1118274B (en)
LU (1) LU80759A1 (en)
NL (1) NL7900207A (en)
NO (1) NO790056L (en)
SE (1) SE7900141L (en)

Cited By (22)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4316777A (en) * 1979-10-01 1982-02-23 Duracell International Inc. Rechargeable nonaqueous silver alloy anode cell
US4330601A (en) * 1979-10-01 1982-05-18 Duracell International Inc. Rechargeable nonaqueous silver alloy anode cell
US4581307A (en) * 1984-03-28 1986-04-08 Saft, S.A. High specific energy electrochemical cell with low initial impedance
US6436583B1 (en) 2000-08-04 2002-08-20 Moltech Corporation Storage life enhancement in lithium-sulfur batteries
US9312522B2 (en) 2012-10-18 2016-04-12 Ambri Inc. Electrochemical energy storage devices
US9502737B2 (en) 2013-05-23 2016-11-22 Ambri Inc. Voltage-enhanced energy storage devices
US9520618B2 (en) 2013-02-12 2016-12-13 Ambri Inc. Electrochemical energy storage devices
US9735450B2 (en) 2012-10-18 2017-08-15 Ambri Inc. Electrochemical energy storage devices
US9893385B1 (en) 2015-04-23 2018-02-13 Ambri Inc. Battery management systems for energy storage devices
US10181800B1 (en) 2015-03-02 2019-01-15 Ambri Inc. Power conversion systems for energy storage devices
US10270139B1 (en) 2013-03-14 2019-04-23 Ambri Inc. Systems and methods for recycling electrochemical energy storage devices
US10541451B2 (en) 2012-10-18 2020-01-21 Ambri Inc. Electrochemical energy storage devices
US10608212B2 (en) 2012-10-16 2020-03-31 Ambri Inc. Electrochemical energy storage devices and housings
US10637015B2 (en) 2015-03-05 2020-04-28 Ambri Inc. Ceramic materials and seals for high temperature reactive material devices
US11211641B2 (en) 2012-10-18 2021-12-28 Ambri Inc. Electrochemical energy storage devices
US11387497B2 (en) 2012-10-18 2022-07-12 Ambri Inc. Electrochemical energy storage devices
US11411254B2 (en) 2017-04-07 2022-08-09 Ambri Inc. Molten salt battery with solid metal cathode
US11721841B2 (en) 2012-10-18 2023-08-08 Ambri Inc. Electrochemical energy storage devices
US11909004B2 (en) 2013-10-16 2024-02-20 Ambri Inc. Electrochemical energy storage devices
US11929466B2 (en) 2016-09-07 2024-03-12 Ambri Inc. Electrochemical energy storage devices
US12142735B1 (en) 2013-11-01 2024-11-12 Ambri, Inc. Thermal management of liquid metal batteries
US12224447B2 (en) 2018-12-17 2025-02-11 Ambri Inc. High temperature energy storage systems and methods

Families Citing this family (3)

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US4315976A (en) * 1979-12-21 1982-02-16 Union Carbide Corporation Coated active anodes
FR2513817B1 (en) * 1981-09-30 1987-02-06 Europ Agence Spatiale IMPROVEMENTS ON BATTERIES
JPH0719609B2 (en) * 1985-07-31 1995-03-06 ソニー株式会社 Organic electrolyte battery

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US3870561A (en) * 1969-10-09 1975-03-11 Battelle Memorial Institute Electric accumulator
US3960594A (en) * 1972-11-09 1976-06-01 Rheinisch-Westfalisches Elektrizitatswerk Aktiengesellschaft Primary or secondary electrochemical cell
US4049892A (en) * 1976-12-27 1977-09-20 Union Carbide Corporation Non-aqueous cell having as cathode a mixture of lead dioxide and lead monoxide and/or lead particles

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FR1189268A (en) * 1957-11-26 1959-10-01 Improvements to batteries and electric accumulators
US3506491A (en) * 1968-05-08 1970-04-14 Standard Oil Co Solid electrolyte battery having lithium or lithium alloy anode
BE791609A (en) * 1971-11-26 1973-05-21 Accumulateurs Fixes CYLINDRICAL ELECTRIC BATTERY
GB1376423A (en) * 1972-05-19 1974-12-04 Mallory & Co Inc P R Organic electrolyte cells with storage life
US3881951A (en) * 1974-07-05 1975-05-06 Rockwell International Corp Lithium electrode and method of producing the same
FR2288401A1 (en) * 1974-10-17 1976-05-14 Accumulateurs Fixes ELECTROCHEMICAL GENERATOR
US4002492A (en) * 1975-07-01 1977-01-11 Exxon Research And Engineering Company Rechargeable lithium-aluminum anode
DE2546585C3 (en) * 1975-10-17 1981-04-16 Varta Batterie Ag, 3000 Hannover Process for the production of galvanic elements with negative electrodes made of lithium or calcium

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3870561A (en) * 1969-10-09 1975-03-11 Battelle Memorial Institute Electric accumulator
US3960594A (en) * 1972-11-09 1976-06-01 Rheinisch-Westfalisches Elektrizitatswerk Aktiengesellschaft Primary or secondary electrochemical cell
US4049892A (en) * 1976-12-27 1977-09-20 Union Carbide Corporation Non-aqueous cell having as cathode a mixture of lead dioxide and lead monoxide and/or lead particles

Cited By (31)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4330601A (en) * 1979-10-01 1982-05-18 Duracell International Inc. Rechargeable nonaqueous silver alloy anode cell
US4316777A (en) * 1979-10-01 1982-02-23 Duracell International Inc. Rechargeable nonaqueous silver alloy anode cell
US4581307A (en) * 1984-03-28 1986-04-08 Saft, S.A. High specific energy electrochemical cell with low initial impedance
US6436583B1 (en) 2000-08-04 2002-08-20 Moltech Corporation Storage life enhancement in lithium-sulfur batteries
US10608212B2 (en) 2012-10-16 2020-03-31 Ambri Inc. Electrochemical energy storage devices and housings
US11211641B2 (en) 2012-10-18 2021-12-28 Ambri Inc. Electrochemical energy storage devices
US11611112B2 (en) 2012-10-18 2023-03-21 Ambri Inc. Electrochemical energy storage devices
US9735450B2 (en) 2012-10-18 2017-08-15 Ambri Inc. Electrochemical energy storage devices
US9825265B2 (en) 2012-10-18 2017-11-21 Ambri Inc. Electrochemical energy storage devices
US11387497B2 (en) 2012-10-18 2022-07-12 Ambri Inc. Electrochemical energy storage devices
US11721841B2 (en) 2012-10-18 2023-08-08 Ambri Inc. Electrochemical energy storage devices
US9312522B2 (en) 2012-10-18 2016-04-12 Ambri Inc. Electrochemical energy storage devices
US10541451B2 (en) 2012-10-18 2020-01-21 Ambri Inc. Electrochemical energy storage devices
US11196091B2 (en) 2012-10-18 2021-12-07 Ambri Inc. Electrochemical energy storage devices
US9520618B2 (en) 2013-02-12 2016-12-13 Ambri Inc. Electrochemical energy storage devices
US9728814B2 (en) 2013-02-12 2017-08-08 Ambri Inc. Electrochemical energy storage devices
US10270139B1 (en) 2013-03-14 2019-04-23 Ambri Inc. Systems and methods for recycling electrochemical energy storage devices
US10297870B2 (en) 2013-05-23 2019-05-21 Ambri Inc. Voltage-enhanced energy storage devices
US9559386B2 (en) 2013-05-23 2017-01-31 Ambri Inc. Voltage-enhanced energy storage devices
US9502737B2 (en) 2013-05-23 2016-11-22 Ambri Inc. Voltage-enhanced energy storage devices
US11909004B2 (en) 2013-10-16 2024-02-20 Ambri Inc. Electrochemical energy storage devices
US12142735B1 (en) 2013-11-01 2024-11-12 Ambri, Inc. Thermal management of liquid metal batteries
US10181800B1 (en) 2015-03-02 2019-01-15 Ambri Inc. Power conversion systems for energy storage devices
US10566662B1 (en) 2015-03-02 2020-02-18 Ambri Inc. Power conversion systems for energy storage devices
US11289759B2 (en) 2015-03-05 2022-03-29 Ambri, Inc. Ceramic materials and seals for high temperature reactive material devices
US11840487B2 (en) 2015-03-05 2023-12-12 Ambri, Inc. Ceramic materials and seals for high temperature reactive material devices
US10637015B2 (en) 2015-03-05 2020-04-28 Ambri Inc. Ceramic materials and seals for high temperature reactive material devices
US9893385B1 (en) 2015-04-23 2018-02-13 Ambri Inc. Battery management systems for energy storage devices
US11929466B2 (en) 2016-09-07 2024-03-12 Ambri Inc. Electrochemical energy storage devices
US11411254B2 (en) 2017-04-07 2022-08-09 Ambri Inc. Molten salt battery with solid metal cathode
US12224447B2 (en) 2018-12-17 2025-02-11 Ambri Inc. High temperature energy storage systems and methods

Also Published As

Publication number Publication date
GB2013020A (en) 1979-08-01
LU80759A1 (en) 1979-09-07
DE2900087A1 (en) 1979-07-12
DE2900087B2 (en) 1981-07-23
ES476726A1 (en) 1979-11-01
BR7900113A (en) 1979-08-14
DK9379A (en) 1979-07-11
SE7900141L (en) 1979-07-11
IT1118274B (en) 1986-02-24
NO790056L (en) 1979-07-11
FR2414253A1 (en) 1979-08-03
GB2013020B (en) 1982-08-18
AU518526B2 (en) 1981-10-01
FR2414253B1 (en) 1981-04-10
DE2900087C3 (en) 1982-04-15
CH630494A5 (en) 1982-06-15
BE873068A (en) 1979-06-27
NL7900207A (en) 1979-07-12
CA1114447A (en) 1981-12-15
AU4318079A (en) 1979-07-19
IT7967040A0 (en) 1979-01-09

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